A pulsed-dc (direct current) magnetron sputtering with a plasma emission monitor (PEM) system was applied to synthesize Cr-containing hydrogenated amorphous diamond-like carbon (Cr-DLC) films using a large-size industrial Cr target. The plasma emission intensity of a Cr atom at 358 nm wavelength was characterized by optical emission spectrometer (OES). C₂H₂ gas flow rate was precisely adjusted to obtain a stable plasma emission intensity. The relationships between Cr atom plasma emission intensity and the element concentration, cross-sectional morphology, deposition rate, microstructure, mechanical properties, and tribological properties of Cr-DLC films were investigated. Scanning electron microscope and Raman spectra were employed to analyze the chemical composition and microstructure, respectively. The mechanical and tribological behaviors were characterized and analyzed by using the nano-indentation, scratch test instrument, and ball-on-disk reciprocating friction/wear tester. The results indicate that the PEM system was successfully used in magnetron sputtering for a more stable Cr-DLC deposition process.